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4-inch Fe doped and S doped InP crystals have been grown by phosphorous vapor controlled LEC method (PC-LEC). By controlling the solid / liquid (SL) interface shape, the dislocation density of S doped InP crystals was reduced to less than 3 × 103 cm-2 for the whole ingot. The dislocation density of 4 inch Fe doped InP crystals was less than 5 × 104 cm-2. The total thickness variation (TTV) of 4-inch substrates was improved by optimizing the polishing conditions. The minimum TTV was about 1.6 micrometer. There was no significant difference in breakage strength between 4-inch and 3-inch Fe doped InP substrates.